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  4. Inexpensive modeling of quantum dynamics using path integral generalized Langevin equation thermostats
 
research article

Inexpensive modeling of quantum dynamics using path integral generalized Langevin equation thermostats

Kapil, Venkat  
•
Wilkins, David M.  
•
Lan, Jinggang
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March 31, 2020
Journal Of Chemical Physics

The properties of molecules and materials containing light nuclei are affected by their quantum mechanical nature. Accurate modeling of these quantum nuclear effects requires computationally demanding path integral techniques. Considerable success has been achieved in reducing the cost of such simulations by using generalized Langevin dynamics to induce frequency-dependent fluctuations. Path integral generalized Langevin equation methods, however, have this far been limited to the study of static, thermodynamic properties due to the large perturbation to the system's dynamics induced by the aggressive thermostatting. Here, we introduce a post-processing scheme, based on analytical estimates of the dynamical perturbation induced by the generalized Langevin dynamics, which makes it possible to recover meaningful time correlation properties from a thermostatted trajectory. We show that this approach yields spectroscopic observables for model and realistic systems that have an accuracy comparable to much more demanding approximate quantum dynamics techniques based on full path integral simulations.

  • Details
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Type
research article
DOI
10.1063/1.5141950
Web of Science ID

WOS:000522036600002

Author(s)
Kapil, Venkat  
Wilkins, David M.  
Lan, Jinggang
Ceriotti, Michele  
Date Issued

2020-03-31

Published in
Journal Of Chemical Physics
Volume

152

Issue

12

Article Number

124104

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

liquid water

•

statistical-mechanics

•

spectroscopy

•

intensity

•

nuclear

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
Available on Infoscience
April 10, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/168089
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